CA2646013A1 - Removal of hg, nox and sox using oxidants and staged gas/liquid contact - Google Patents
Removal of hg, nox and sox using oxidants and staged gas/liquid contact Download PDFInfo
- Publication number
- CA2646013A1 CA2646013A1 CA002646013A CA2646013A CA2646013A1 CA 2646013 A1 CA2646013 A1 CA 2646013A1 CA 002646013 A CA002646013 A CA 002646013A CA 2646013 A CA2646013 A CA 2646013A CA 2646013 A1 CA2646013 A1 CA 2646013A1
- Authority
- CA
- Canada
- Prior art keywords
- set forth
- sodium
- compounds
- oxidant
- gas
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Abandoned
Links
- 239000007800 oxidant agent Substances 0.000 title claims abstract description 54
- 239000007788 liquid Substances 0.000 title description 6
- 238000000034 method Methods 0.000 claims abstract description 79
- 239000007789 gas Substances 0.000 claims abstract description 59
- 230000001590 oxidative effect Effects 0.000 claims abstract description 39
- 150000001875 compounds Chemical class 0.000 claims abstract description 36
- 229910052753 mercury Inorganic materials 0.000 claims abstract description 28
- 238000005201 scrubbing Methods 0.000 claims abstract description 25
- 239000002594 sorbent Substances 0.000 claims abstract description 18
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 51
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 claims description 51
- 239000000243 solution Substances 0.000 claims description 41
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 39
- UIIMBOGNXHQVGW-UHFFFAOYSA-M Sodium bicarbonate Chemical compound [Na+].OC([O-])=O UIIMBOGNXHQVGW-UHFFFAOYSA-M 0.000 claims description 24
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 claims description 20
- 238000002347 injection Methods 0.000 claims description 19
- 239000007924 injection Substances 0.000 claims description 19
- 235000011121 sodium hydroxide Nutrition 0.000 claims description 17
- 229910001868 water Inorganic materials 0.000 claims description 15
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 14
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 14
- 229910017604 nitric acid Inorganic materials 0.000 claims description 14
- 229910000030 sodium bicarbonate Inorganic materials 0.000 claims description 13
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 12
- 239000011734 sodium Substances 0.000 claims description 12
- 229910052708 sodium Inorganic materials 0.000 claims description 12
- 235000017557 sodium bicarbonate Nutrition 0.000 claims description 12
- 229910000029 sodium carbonate Inorganic materials 0.000 claims description 12
- 239000003513 alkali Substances 0.000 claims description 11
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 10
- BZSXEZOLBIJVQK-UHFFFAOYSA-N 2-methylsulfonylbenzoic acid Chemical compound CS(=O)(=O)C1=CC=CC=C1C(O)=O BZSXEZOLBIJVQK-UHFFFAOYSA-N 0.000 claims description 9
- 239000002253 acid Substances 0.000 claims description 9
- 239000012286 potassium permanganate Substances 0.000 claims description 9
- XTEGARKTQYYJKE-UHFFFAOYSA-N chloric acid Chemical compound OCl(=O)=O XTEGARKTQYYJKE-UHFFFAOYSA-N 0.000 claims description 8
- 229940005991 chloric acid Drugs 0.000 claims description 8
- OSVXSBDYLRYLIG-UHFFFAOYSA-N dioxidochlorine(.) Chemical compound O=Cl=O OSVXSBDYLRYLIG-UHFFFAOYSA-N 0.000 claims description 8
- 235000017550 sodium carbonate Nutrition 0.000 claims description 7
- SUKJFIGYRHOWBL-UHFFFAOYSA-N sodium hypochlorite Chemical compound [Na+].Cl[O-] SUKJFIGYRHOWBL-UHFFFAOYSA-N 0.000 claims description 7
- 239000000654 additive Substances 0.000 claims description 6
- UKLNMMHNWFDKNT-UHFFFAOYSA-M sodium chlorite Chemical compound [Na+].[O-]Cl=O UKLNMMHNWFDKNT-UHFFFAOYSA-M 0.000 claims description 6
- 229960002218 sodium chlorite Drugs 0.000 claims description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 6
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 claims description 5
- 239000005708 Sodium hypochlorite Substances 0.000 claims description 5
- 230000001143 conditioned effect Effects 0.000 claims description 5
- 239000004155 Chlorine dioxide Substances 0.000 claims description 4
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 claims description 4
- 239000006172 buffering agent Substances 0.000 claims description 4
- 235000019398 chlorine dioxide Nutrition 0.000 claims description 4
- 150000007524 organic acids Chemical class 0.000 claims description 4
- 235000005985 organic acids Nutrition 0.000 claims description 4
- 230000003647 oxidation Effects 0.000 claims description 4
- 238000007254 oxidation reaction Methods 0.000 claims description 4
- 239000011591 potassium Substances 0.000 claims description 4
- 229910052700 potassium Inorganic materials 0.000 claims description 4
- VKJKEPKFPUWCAS-UHFFFAOYSA-M potassium chlorate Chemical compound [K+].[O-]Cl(=O)=O VKJKEPKFPUWCAS-UHFFFAOYSA-M 0.000 claims description 4
- SATVIFGJTRRDQU-UHFFFAOYSA-N potassium hypochlorite Chemical compound [K+].Cl[O-] SATVIFGJTRRDQU-UHFFFAOYSA-N 0.000 claims description 4
- VISKNDGJUCDNMS-UHFFFAOYSA-M potassium;chlorite Chemical compound [K+].[O-]Cl=O VISKNDGJUCDNMS-UHFFFAOYSA-M 0.000 claims description 4
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 3
- 239000000539 dimer Substances 0.000 claims description 3
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 claims 6
- UIIMBOGNXHQVGW-DEQYMQKBSA-M Sodium bicarbonate-14C Chemical compound [Na+].O[14C]([O-])=O UIIMBOGNXHQVGW-DEQYMQKBSA-M 0.000 claims 3
- 229910000019 calcium carbonate Inorganic materials 0.000 claims 3
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 claims 3
- 239000000920 calcium hydroxide Substances 0.000 claims 3
- 229910001861 calcium hydroxide Inorganic materials 0.000 claims 3
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 claims 3
- 239000000292 calcium oxide Substances 0.000 claims 3
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims 3
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 claims 3
- 239000001095 magnesium carbonate Substances 0.000 claims 3
- 229910000021 magnesium carbonate Inorganic materials 0.000 claims 3
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 claims 3
- 239000000347 magnesium hydroxide Substances 0.000 claims 3
- 229910001862 magnesium hydroxide Inorganic materials 0.000 claims 3
- 239000000395 magnesium oxide Substances 0.000 claims 3
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims 3
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims 3
- 230000003134 recirculating effect Effects 0.000 claims 2
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 abstract description 86
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical class [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 abstract description 14
- 150000002731 mercury compounds Chemical class 0.000 abstract 2
- 239000003546 flue gas Substances 0.000 description 27
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 26
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 23
- 238000006243 chemical reaction Methods 0.000 description 18
- 239000003153 chemical reaction reagent Substances 0.000 description 12
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 description 11
- 229910021529 ammonia Inorganic materials 0.000 description 11
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 11
- AKEJUJNQAAGONA-UHFFFAOYSA-N sulfur trioxide Chemical compound O=S(=O)=O AKEJUJNQAAGONA-UHFFFAOYSA-N 0.000 description 11
- 239000000356 contaminant Substances 0.000 description 10
- 229910052815 sulfur oxide Inorganic materials 0.000 description 10
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 8
- 229910002089 NOx Inorganic materials 0.000 description 7
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 description 7
- 229910052938 sodium sulfate Inorganic materials 0.000 description 7
- 235000011152 sodium sulphate Nutrition 0.000 description 7
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical class S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 description 7
- 238000005200 wet scrubbing Methods 0.000 description 7
- 238000013459 approach Methods 0.000 description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 5
- 238000012546 transfer Methods 0.000 description 5
- 238000010521 absorption reaction Methods 0.000 description 4
- 230000008901 benefit Effects 0.000 description 4
- 238000002485 combustion reaction Methods 0.000 description 4
- 238000002156 mixing Methods 0.000 description 4
- 239000011780 sodium chloride Substances 0.000 description 4
- 239000007921 spray Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 3
- 235000019738 Limestone Nutrition 0.000 description 3
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 3
- 239000007832 Na2SO4 Substances 0.000 description 3
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 3
- 239000012670 alkaline solution Substances 0.000 description 3
- 239000012298 atmosphere Substances 0.000 description 3
- 239000011575 calcium Substances 0.000 description 3
- 229910052791 calcium Inorganic materials 0.000 description 3
- 238000010531 catalytic reduction reaction Methods 0.000 description 3
- 239000000446 fuel Substances 0.000 description 3
- 239000006028 limestone Substances 0.000 description 3
- 239000011777 magnesium Substances 0.000 description 3
- 229910052749 magnesium Inorganic materials 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 239000000376 reactant Substances 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 239000012719 wet electrostatic precipitator Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 2
- 235000008733 Citrus aurantifolia Nutrition 0.000 description 2
- 229910020939 NaC104 Inorganic materials 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 235000011941 Tilia x europaea Nutrition 0.000 description 2
- 239000006096 absorbing agent Substances 0.000 description 2
- 231100001245 air toxic agent Toxicity 0.000 description 2
- BIGPRXCJEDHCLP-UHFFFAOYSA-N ammonium bisulfate Chemical compound [NH4+].OS([O-])(=O)=O BIGPRXCJEDHCLP-UHFFFAOYSA-N 0.000 description 2
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 description 2
- 229910052921 ammonium sulfate Inorganic materials 0.000 description 2
- 235000011130 ammonium sulphate Nutrition 0.000 description 2
- 238000011021 bench scale process Methods 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000001311 chemical methods and process Methods 0.000 description 2
- 238000012993 chemical processing Methods 0.000 description 2
- 239000007795 chemical reaction product Substances 0.000 description 2
- 239000000567 combustion gas Substances 0.000 description 2
- 238000011109 contamination Methods 0.000 description 2
- 238000005203 dry scrubbing Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 239000002803 fossil fuel Substances 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 2
- 239000004571 lime Substances 0.000 description 2
- 150000002823 nitrates Chemical class 0.000 description 2
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 2
- 238000012856 packing Methods 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- FGIUAXJPYTZDNR-UHFFFAOYSA-N potassium nitrate Chemical compound [K+].[O-][N+]([O-])=O FGIUAXJPYTZDNR-UHFFFAOYSA-N 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 238000006722 reduction reaction Methods 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 235000015424 sodium Nutrition 0.000 description 2
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 2
- 238000005507 spraying Methods 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 235000011149 sulphuric acid Nutrition 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-M Bisulfite Chemical compound OS([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-M 0.000 description 1
- KZBUYRJDOAKODT-UHFFFAOYSA-N Chlorine Chemical compound ClCl KZBUYRJDOAKODT-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- -1 NO2 Chemical class 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- 229910019093 NaOCl Inorganic materials 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
- IOVCWXUNBOPUCH-UHFFFAOYSA-M Nitrite anion Chemical compound [O-]N=O IOVCWXUNBOPUCH-UHFFFAOYSA-M 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 description 1
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 1
- 239000002250 absorbent Substances 0.000 description 1
- 230000002745 absorbent Effects 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 239000007844 bleaching agent Substances 0.000 description 1
- 238000007664 blowing Methods 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 235000001465 calcium Nutrition 0.000 description 1
- 239000004202 carbamide Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 239000013065 commercial product Substances 0.000 description 1
- 230000003750 conditioning effect Effects 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 239000004035 construction material Substances 0.000 description 1
- 230000002939 deleterious effect Effects 0.000 description 1
- 238000002848 electrochemical method Methods 0.000 description 1
- 239000012717 electrostatic precipitator Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003337 fertilizer Substances 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- ZZUFCTLCJUWOSV-UHFFFAOYSA-N furosemide Chemical compound C1=C(Cl)C(S(=O)(=O)N)=CC(C(O)=O)=C1NCC1=CC=CO1 ZZUFCTLCJUWOSV-UHFFFAOYSA-N 0.000 description 1
- 238000010574 gas phase reaction Methods 0.000 description 1
- 239000008246 gaseous mixture Substances 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 1
- 239000002440 industrial waste Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000005184 irreversible process Methods 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 235000001055 magnesium Nutrition 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000010297 mechanical methods and process Methods 0.000 description 1
- 229910000474 mercury oxide Inorganic materials 0.000 description 1
- 239000003595 mist Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 238000010979 pH adjustment Methods 0.000 description 1
- 150000002978 peroxides Chemical class 0.000 description 1
- 238000005498 polishing Methods 0.000 description 1
- 235000010333 potassium nitrate Nutrition 0.000 description 1
- 239000004323 potassium nitrate Substances 0.000 description 1
- 229910052939 potassium sulfate Inorganic materials 0.000 description 1
- 238000007430 reference method Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000005070 sampling Methods 0.000 description 1
- 238000012216 screening Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 230000035945 sensitivity Effects 0.000 description 1
- 239000010802 sludge Substances 0.000 description 1
- HYHCSLBZRBJJCH-UHFFFAOYSA-M sodium hydrosulfide Chemical compound [Na+].[SH-] HYHCSLBZRBJJCH-UHFFFAOYSA-M 0.000 description 1
- 235000010344 sodium nitrate Nutrition 0.000 description 1
- 239000004071 soot Substances 0.000 description 1
- 238000001694 spray drying Methods 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 150000004763 sulfides Chemical class 0.000 description 1
- 150000003464 sulfur compounds Chemical class 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 239000004753 textile Substances 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
- 238000004065 wastewater treatment Methods 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/48—Sulfur compounds
- B01D53/50—Sulfur oxides
- B01D53/501—Sulfur oxides by treating the gases with a solution or a suspension of an alkali or earth-alkali or ammonium compound
- B01D53/504—Sulfur oxides by treating the gases with a solution or a suspension of an alkali or earth-alkali or ammonium compound characterised by a specific device
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1406—Multiple stage absorption
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1456—Removing acid components
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/48—Sulfur compounds
- B01D53/50—Sulfur oxides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/48—Sulfur compounds
- B01D53/50—Sulfur oxides
- B01D53/501—Sulfur oxides by treating the gases with a solution or a suspension of an alkali or earth-alkali or ammonium compound
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
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- F23J15/00—Arrangements of devices for treating smoke or fumes
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Abstract
A method of scrubbing mercury compounds and nitrogen oxides from a gas stream employing a scrubbing operation. The method involves the contact of the stream which contains mercury, SOx and NOx compounds with a sorbent to remove at least a portion of the latter compounds. This results in a partially cleaned stream. The method further involves contacting the latter stream with an oxidant to oxidize and remove substantially all residual nitrogen oxides, mercury and mercury compounds remaining in the stream.
Description
REMOVAL OF Hg, NOx, AND SOX USING
OXIDANTS AND STAGED GAS/LIQUID CONTACT
[0001] This application claims priority to U.S. Patent Application Serial No. 11/081,612, filed March 17, 2005.
FIELD OF THE INVENTION
OXIDANTS AND STAGED GAS/LIQUID CONTACT
[0001] This application claims priority to U.S. Patent Application Serial No. 11/081,612, filed March 17, 2005.
FIELD OF THE INVENTION
[0002] The present invention relates to removal of SOX and NOX and mercury with oxidants, and more particularly, the present invention relates to removal of SOx, NOx, and Hg with staged gas/liquid contact.
BACKGROUND OF THE INVENTION
BACKGROUND OF THE INVENTION
[0003] In the pollution control field, several approaches are used to remove sulfur oxides and other contaminants from a flue gas produced by the burning of a fossil fuel in order to comply with Federal and State emissions requirements. One approach involves locating and utilizing fossil fuels lower in sulfur content and/or other contaminants. A second approach involves removing or reducing the sulfur content and/or other contaminants in the fuel, prior to combustion, via mechanical and/or chemical processes. A
major disadvantage to the second approach is the limited cost effectiveness of the mechanical and/or chemical processing required to achieve the mandated reduction levels of sulfur oxides and/or other contaminants.
major disadvantage to the second approach is the limited cost effectiveness of the mechanical and/or chemical processing required to achieve the mandated reduction levels of sulfur oxides and/or other contaminants.
[0004] By and large, the most widely used approaches to removing sulfur oxides and/or other contaminants from flue gas involve post-combustion clean up of the flue gas. Several methods have been developed to remove the SOz species from flue gases.
[0005] A first method for removing SO2 from flue gas involves either mixing dry alkali material with the fuel prior to combustion, or injection of pulverized alkali material directly into the hot combustion gases to remove sulfur oxides and other contaminants U: W I I S ta f f\c a Id we l l\S c a n-1. doc via absorption or absorption followed by oxidation. Major disadvantages of this first method include: fouling of heat transfer surfaces (which then requires more frequent soot blowing of these heat transfer surfaces), low to moderate removal efficiencies, poor reagent utilization, and increased particulate loading in the combustion gases which may require additional conditioning (i.e. humidification or sulfur trioxide injection) of the gas if an electrostatic precipitator is used for downstream particulate collection.
[0006] A second method for removing SOz from flue gas, collectively referred to as wet chemical absorption processes and also known as wet scrubbing, involves "washing" the hot flue gases with an aqueous alkaline solution or slurry in a gas-liquid contact device to remove sulfur oxides and other contaminants. Major disadvantages associated with these wet scrubbing prbcesses include: the loss of liquid both to the atmosphere (i.e., due to saturation of the flue gas and mist carry-over) and to the sludge produced in the process; and the economics associated with the construction materials for the absorber module itself and all related auxiliary downstream equipment (i.e., primary/secondary dewatering and waste water treatment subsystems). A typical wet scrubbing system is shown in Figure 1.
[0007]A third method, collectively referred to as spray drying chemical absorption processes and also known as dry scrubbing, involves spraying an aqueous alkaline solution or slurry which has been finely atomized via mechanical, dual-fluid or rotary type atomizers, into the hot flue gases to remove sulfur oxides and other contaminants. Major disadvantages associated with these dry scrubbing processes include: moderate to high gas-side pressure drop across the spray dryer gas inlet distribution device, and limitations on the spray down temperature (i.e., the approach to flue gas saturation temperature) required to maintain controlled operations.
[0008] There are several methods forcontrolling NOX emissions.
Selective Catalytic Reduction (SCR) is the most common method. In these processes, ammonia is injected and mixed with the flue gas at low to medium temperatures. The mixture then flows across a catalyst (often vanadium based over a stainless steel substrate)and the NOX is reduced to N2. The problems with SCR
systems is the high initial cost, high cost of ammonia which is thermally or chemically decomposed, and the introduction of ammonia into the gas stream causing problems with the formation of ammonium bisulfate and ammonia slip the atmosphere. Selective Non-catalytic Reduction (SNCR) methods are also employed. In these processes ammonia or urea is injected into hot flue gases resulting with a direct reaction forming N2. The problems with SNCR
systems is the challenges with mixing and maintaining proper residence time and operating conditions for the reactions to take place optimally, sensitivity to changes in operating load, the high cost of ammonia which is thermally or chemically decomposed (even more, than SCRs), and the introduction of ammonia into the gas stream causing problems with the formation of ammonium bisulfate and ammonia slip (as high as 50 ppm or higher) to the atmosphere.
Selective Catalytic Reduction (SCR) is the most common method. In these processes, ammonia is injected and mixed with the flue gas at low to medium temperatures. The mixture then flows across a catalyst (often vanadium based over a stainless steel substrate)and the NOX is reduced to N2. The problems with SCR
systems is the high initial cost, high cost of ammonia which is thermally or chemically decomposed, and the introduction of ammonia into the gas stream causing problems with the formation of ammonium bisulfate and ammonia slip the atmosphere. Selective Non-catalytic Reduction (SNCR) methods are also employed. In these processes ammonia or urea is injected into hot flue gases resulting with a direct reaction forming N2. The problems with SNCR
systems is the challenges with mixing and maintaining proper residence time and operating conditions for the reactions to take place optimally, sensitivity to changes in operating load, the high cost of ammonia which is thermally or chemically decomposed (even more, than SCRs), and the introduction of ammonia into the gas stream causing problems with the formation of ammonium bisulfate and ammonia slip (as high as 50 ppm or higher) to the atmosphere.
[0009] NOx removal through injection of sodium bicarbonate (NaHCO3) has been demonstrated by NaTec and others.
[0010] In the prior art for wet chemical NOx reduction, the use of oxidants such as hydrogen peroxide is employed. Hydrogen peroxide is an oxidizing agent for organic and inorganic chemical processing as well as semi-conductor, applications bleach for textiles and pulp, and a treatment for municipal and industrial waste. Hydrogen Peroxide (H202) is an effective means of scrubbing Nitrogen Oxides. It has been used for many years. The use of H202 and HN03 to scrub both NO and NO2 is an attractive option because the combination handles widely varying rates of NO to NO2, adds no contaminants to the scrubbing solution or blow-down/waste stream and allows a commercial product to be recovered from the process, i.e. nitric acid or ammonium nitrate.
UWIStaff\caldwelllScan- ] .doc [0011] Gas scrubbing is another common form of NO;, treatment, with sodium hydroxide being the conventional scrubbing medium. However, the absorbed NOx is converted to nitrite and nitrate which may present wastewater disposal problems. Scrubbing solutions containing hydrogen peroxide are also effective at removing NO,, and can afford benefits not available with NaOH. For example, H202 adds no contaminants to the scrubbing solution and so allows commercial products to be recovered from the process, e.g., nitric acid. In its simplest application, H202 and nitric acid are used to scrub both nitric oxide (NO) and nitrogen dioxide (NO2) - the chief components of NOX from many utility and industrial sources.
UWIStaff\caldwelllScan- ] .doc [0011] Gas scrubbing is another common form of NO;, treatment, with sodium hydroxide being the conventional scrubbing medium. However, the absorbed NOx is converted to nitrite and nitrate which may present wastewater disposal problems. Scrubbing solutions containing hydrogen peroxide are also effective at removing NO,, and can afford benefits not available with NaOH. For example, H202 adds no contaminants to the scrubbing solution and so allows commercial products to be recovered from the process, e.g., nitric acid. In its simplest application, H202 and nitric acid are used to scrub both nitric oxide (NO) and nitrogen dioxide (NO2) - the chief components of NOX from many utility and industrial sources.
[0012] There are several other processes which also use hydrogen peroxide to remove NOX. The Kanto Denka process employs a scrubbing solution containing 0.2% hydrogen peroxide and 10%
nitric acid while the Nikon process uses a 10% sodium hydroxide solution containing 3.5% hydrogen peroxide. A fourth process, the Ozawa process, scrubs NOX by spraying a hydrogen peroxide solution into the exhaust gas stream. The liquid is then separated from the gas stream, and the nitric acid formed is neutralized with potassium hydroxide. The excess potassium nitrate is crystallized out, and the solution reused after recharging with hydrogen. In addition to the methods cited above in which NOX is oxidized to nitric acid or nitrate salts, a series of Japanese patents describe processes and equipment for reducing NOX to nitrogen using hydrogen peroxide and ammonia.
nitric acid while the Nikon process uses a 10% sodium hydroxide solution containing 3.5% hydrogen peroxide. A fourth process, the Ozawa process, scrubs NOX by spraying a hydrogen peroxide solution into the exhaust gas stream. The liquid is then separated from the gas stream, and the nitric acid formed is neutralized with potassium hydroxide. The excess potassium nitrate is crystallized out, and the solution reused after recharging with hydrogen. In addition to the methods cited above in which NOX is oxidized to nitric acid or nitrate salts, a series of Japanese patents describe processes and equipment for reducing NOX to nitrogen using hydrogen peroxide and ammonia.
[0013] Also worth mentioning is the fact that H202 is used for the measurement of Nitrogen Oxide in the Standard Reference Method 7 of the Code of Federal Regulations (CFR) promulgated test methods published in the Federal Register as final rules by the US
Environmental Protection Agency (EPA). In this procedure, an H202 solution is used in a flask to effectively capture the NOX. This, however is a slow reaction that requires several hours to complete.
Environmental Protection Agency (EPA). In this procedure, an H202 solution is used in a flask to effectively capture the NOX. This, however is a slow reaction that requires several hours to complete.
[0014] There are two primary reasons that H2O2 has not gained widespread use as a reagent for removal of NO,, in utility and large industrial applications. The first is that it is not a selective oxidant. Most of these sources also contain other species, primarily, SOz which are also effectively removed with hydrogen peroxide. Thus, a large quantity of H202 would be required compared to the amount of NOX removal sought. Even after a limestone scrubber, the amount of SO2 present in flue gas may be equal to or greater than the amount of NO,.
[0015] The second reason that H202 has not gained widespread use is the cost, especially when much more is required due to reactions with SO2, for example, which can be better done prior to the H202 stage.
The overall reactions are:
1) 3H202 + 2NO -~ 2HN03 + 2H20 2) H202 + 2N02 -~ 2HN03 3) H202 + SO2 -~ H2SO4 [0016] Oxidation utilizing gases have been demonstrated in the art.
It has been shown that over 90% of gas phase NO can be converted to NO2 rapidly by C102 at an applied rate of approximately 1.2 kg C102/kg NO. This of course requires proper mixing conditions. C102 is a much stronger oxidizer than hydrogen peroxide, sodium chlorate or sodium chlorite and would be a preferred oxidizer.
Ozone is also a possibility, but has orders of magnitude greater capital costs relative to C102 generators.
The overall reactions are:
1) 3H202 + 2NO -~ 2HN03 + 2H20 2) H202 + 2N02 -~ 2HN03 3) H202 + SO2 -~ H2SO4 [0016] Oxidation utilizing gases have been demonstrated in the art.
It has been shown that over 90% of gas phase NO can be converted to NO2 rapidly by C102 at an applied rate of approximately 1.2 kg C102/kg NO. This of course requires proper mixing conditions. C102 is a much stronger oxidizer than hydrogen peroxide, sodium chlorate or sodium chlorite and would be a preferred oxidizer.
Ozone is also a possibility, but has orders of magnitude greater capital costs relative to C102 generators.
[0017] Sulfur dioxide reacts with chlorine dioxide in the gas phase to form sulfuric and hydrochloric acid.
4) 2C102 + 5SO2 + 6H2O ----> 5H2SO4 + 2HC1 [0018] Assuming SO2 is the dominant species in the C10Z reaction in the presence of S02 and NO, then it is advisable, according to this invention, to add C102 after having scrubbed out SOx to keep the economics of adding C102 good.
4) 2C102 + 5SO2 + 6H2O ----> 5H2SO4 + 2HC1 [0018] Assuming SO2 is the dominant species in the C10Z reaction in the presence of S02 and NO, then it is advisable, according to this invention, to add C102 after having scrubbed out SOx to keep the economics of adding C102 good.
[0019]A different process employs a proprietary oxidizing compound plus dilute sulfuric acid in a first stage and an irreversible process involving proprietary solutions and chemistries in a second stage. The system operates at greater than 99% efficiency on both NO and NO2 and will accommodate ambient temperature gas streams.
[0020]The prior art also does not teach simultaneous removal of mercury and NO,, especially elemental mercury (Hg ) removal. The prior art does teach limited capture of mercury using activated carbon and capture of oxidized mercury (Hg+2 such as in the form of HgC12) (United States Patent No. 6,503,470 to Nolan, et al.) in wet scrubbers that use an alkali reagent. This process also uses additives such as sodium hydrogen sulfide (NaHS) or other sulfides to chemically bind with the mercury to form compounds such as HgS.
SUNIlLARY OF THE INVENTION
SUNIlLARY OF THE INVENTION
[0021]One object of one embodiment of the present invention is to provide an improved method for scrubbing flue gas streams.
[0022]A further object of one embodiment of the present invention is to provide a method of scrubbing Hg compounds from a flue gas stream, comprising a scrubbing operation, including: contacting a flue gas stream containing Hg, SO, and NOX compounds with a sorbent for removing at least a portion of said SO., Hg and NO, compounds present in said stream to provide a partially cleaned flue gas stream; and contacting said partially cleaned flue gas stream with an oxidant to oxidize and capture substantially all residual Hg remaining in said stream.
[0023]Yet another object of one embodiment of the present invention is to provide a method of scrubbing NO,t compounds from a flue gas stream containing said NO, compounds, a scrubbing operation, including: contacting a flue gas stream containing SOx and NOX
compounds with a sorbent for removing at least a portion of said SOX and NO,, compounds present in said stream to provide a partially cleaned flue gas stream; and contacting said partially cleaned flue gas stream with an oxidant to oxidize and capture substantially all residual NOX remaining in said stream.
compounds with a sorbent for removing at least a portion of said SOX and NO,, compounds present in said stream to provide a partially cleaned flue gas stream; and contacting said partially cleaned flue gas stream with an oxidant to oxidize and capture substantially all residual NOX remaining in said stream.
[0024] A host of advantages are realized by practicing the methodology of the invention. One advantage is that a high removal of SOz and NO,,(NO, NOZ, and dimers) is achieved with essentially all of the acid gas and air toxics (including NOX) in the flue gas being removed. Particularly convenient is the fact that NOX is removed without the use of ammonia and no SCR
(Selective Catalytic Reduction) system is required for NOX removal.
The methodology also results in the high removal of Hg without the use of expensive activated carbon systems; in the preferred embodiment, all emissions removal is accomplished in a single, staged tower.
(Selective Catalytic Reduction) system is required for NOX removal.
The methodology also results in the high removal of Hg without the use of expensive activated carbon systems; in the preferred embodiment, all emissions removal is accomplished in a single, staged tower.
[0025] It has been found that the oxidant will also effectively remove any SO2 in the flue gas with the overall cost of this ultra high removal system being lower than a system with multiple vessels.
[0026] in terms of other features, less physical space is required than conventional multi-step processes which would employ separate vessels and much more equipment in the gas stream; the amount of oxidant required is reduced, since almost all the sulfur compounds and some of the NOX and Hg are removed prior to the oxidant stage.
[0027] The process permits many choices for reagents for SO2 control in the first add-on stage with sodium alkalis being the preferred reagents due to gas phase reactions in the stage, production of sodium sulfate, the ability to regenerate the sodium alkali, and conveniently, carbon injection equipment is not required as Hg and other air toxics are removed by the staged process steps.
[0028]Further advantages include: each stage can be custom designed to meet the pollutant removal characteristics of the constituents removed in each individual stage; the chemistry of each stage is independently controlled and monitored to optimize the performance; each stage is isolated to prevent contamination of reagents/solutions; and the solutions in each stage are handled separately.
[0029]Having thus described the invention, reference will now be made to the accompanying drawings illustrating preferred embodiments.
BRIEF DESCRIPTION OF THE DRAWINGS
BRIEF DESCRIPTION OF THE DRAWINGS
[0030]Figure 1 is a prior art scrubber arrangement;
[0031]Figure 2 is a scrubber arrangement according to the present invention;
[0032] Figure 3 is a prior scrubber arrangement incorporating a wet electrostatic precipitator (WESP) for the purpose of removing condensables, like H2S04 which forms from SO3 gas and water;
[0033]Figure 4 is a graphical representation of data in accordance with the present invention; and [0034]Figure 5 is a further graphical representation of data in accordance with the present invention.
DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS
DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS
[0035]Wet scrubbing systems such as that shown on Figure 1 and globally denoted by numeral 10 use lime, limestone, soda ash, sodium, magnesium, and calcium or other compounds for scrubbing.
They also can employ any of a number of additives to enhance removal, control chemistry, and reduce chemical scale. These systems are adequate at removing SOz up to maybe 90 - 98%, but do not effectively remove NO, or Hg.
They also can employ any of a number of additives to enhance removal, control chemistry, and reduce chemical scale. These systems are adequate at removing SOz up to maybe 90 - 98%, but do not effectively remove NO, or Hg.
[0036] In the combined system of the present invention, the flue gas is scrubbed by wet scrubbing using prior art technologies like that shown on Figure 1 for partial removal of SO2 (partial removal means less than 100% or typically 90 - 95% such as is known in the prior art for calcium based scrubbers).
[0037] The gas could be, optionally, conditioned by injection of absorbents, reagents, or sorbents to reduce a portion of the inlet SO3. Some sulfur dioxide, hydrochloric acid, NO, or other acid gases may also be removed by the injection. This can be by wet or dry injection with almost any alkali at any of several possible and known locations or temperature zones from the source of the flue gas to the scrubber inlet. However, dry sodium bicarbonate injection is preferred since it will react with the S03, NOX and SO2 and other acid gasses including HC1, HF, H2S, etc. in the gas stream. When injection of sorbents is employed, the need for a wet electrostatic precipitator such as that shown on Figure 3 is eliminated. H2SO4 is not formed since S03 is effectively removed upstream of the wet scrubbing system.
[0038]Following the optional injection step, S02 and acidic NO,, compounds such as NO2, N203 and N205 and their associated dimmers, i.e. N204 are removed in the wet scrubber. In the prior art with sodium bicarbonate injection, the conversion of NO to NOZ was considered undesirable since the NOz was a brown gas that was not captured by the downstream equipment. In this case, the wet scrubber effectively captures some of the NO2, N205, etc. Some of the NO is captured directly by the sodium bicarbonate.
[0039]In the prior art, including United States Patent No. 6,143,263 and United States Patent No. 6,303,083, Method and System for S02 and SO3 Control by Dry Sorbent/Reagent Injection.and Wet Scrubbing, there is no teaching for NOX removal in any form as the NO, is known to be primarily in the form of NO which is not effectively captured with conventional based sorbents such as lime, limestone, or sodium.
[0040] The present invention is a one to three step add-on technology. This applies to all scrubbing systems for gases that contain SOz, NOX, and Hg such as from the combustion of coal or other industrial fuels or from chemical processes. This also applies to both new applications or modifications of existing units.
[0041]For the one stage add-on step, all or almost all SOZ is removed by the prior art system such as a high efficiency scrubber that employs a reagent based on sodium, magnesium, buffered calcium, etc. High removal of SO2 is not necessary, but is preferred. If the SO2 removal is low, then it will be removed by the oxidant. This will require a significant quantity of a higher cost reactant.
[0042] For a 2-stage add-on step, the first a stage is added to effectively remove all or almost all of the remaining SO2. This uses a tray like a bubble cap tray (not shown) or a separate vessel (not shown) to keep the 2"d-stage SO2 reagent stream separate from the lower stage acid gas absorber stage. This is done 'preferably, using a soluble scrubbing solution such as a sodium or magnesium based reagent (hydroxide, carbonate, sulfite, bicarbonate, bisulfite, etc. and may include buffering agents, additives, organic acids, etc.) with the appropriate mass transfer surfaces including any combination of sprays, packing, trays, etc.
[0043] Therefore, for both cases, all or almost all of the SO2 is removed prior to the oxidant stage.
[0044] In the oxidant stage, NOX (primarily in the form of NO, NOz, or other dimers) and mercury (elemental and oxidized) are removed.
Like the first stage of the 2-stage add-on step, this uses a tray like a bubble cap tray or a separate vessel (neither of which are shown) to keep the reagent, in this case an oxidant stream, separate from the lower stages. Mass transfer surfaces such as additional trays, sprays or packing are added as required. The result is that the gas leaving this stage is essentially free of all SOX and has at up to 90% or more of the mercury and NOX
removed. This eliminates Hg, SOX, and NOX contamination in the final stage.
Like the first stage of the 2-stage add-on step, this uses a tray like a bubble cap tray or a separate vessel (neither of which are shown) to keep the reagent, in this case an oxidant stream, separate from the lower stages. Mass transfer surfaces such as additional trays, sprays or packing are added as required. The result is that the gas leaving this stage is essentially free of all SOX and has at up to 90% or more of the mercury and NOX
removed. This eliminates Hg, SOX, and NOX contamination in the final stage.
[0045] An optional add-on stage is used as a final wash. This would be used to make sure any byproduct from the oxidant such as chlorine gas, NO2, etc. is washed from the flue gas. The final wash, if required, would be with water or an appropriate solution.
[0046] A preferred embodiment (see Figure 4) therefore consists of 2 to 5 or more stages. In a five stage system, the first stage is a dry injection step. The second stage is the wet acid gas scrubber using conventional steps known in the art and denoted by numeral 12. The third stage is a polishing step to remove the remaining SO2. The preferred embodiment of the third stage (first add-on stage) is a reaction zone that uses a sodium carbonate (NazCO3), caustic soda (NaOH) or sodium bicarbonate (NaHCO3) reactant. This would produce sodium sulfate by the following overall reactions:
5) 2NaHCO3 + SOZ +1/z02 -~ Na2SO4 + 2CO2r+ H2O
6) Na2C03 + SO2 + 1h0z -1 Na2SO4 + COZ T+ H20 7) 2NaOH + SO2 +~/z02 -~ Na2SO4 + H20 [0047] The sodium carbonate, caustic soda, or sodium bicarbonate (or other reactants) can be purchased. Sodium bicarbonate can be regenerated on site using the processes developed by Airborne Pollution Control. Caustic soda can be produced on site using electrochemical methods from sodium sulfate. In this case, sodium sulfate is split and reacted with ammonia to produce NaOH and (NH4)2SO4. The NaOH is used in the scrubber and the (NH4)2SO4 can be sold as a fertilizer.
5) 2NaHCO3 + SOZ +1/z02 -~ Na2SO4 + 2CO2r+ H2O
6) Na2C03 + SO2 + 1h0z -1 Na2SO4 + COZ T+ H20 7) 2NaOH + SO2 +~/z02 -~ Na2SO4 + H20 [0047] The sodium carbonate, caustic soda, or sodium bicarbonate (or other reactants) can be purchased. Sodium bicarbonate can be regenerated on site using the processes developed by Airborne Pollution Control. Caustic soda can be produced on site using electrochemical methods from sodium sulfate. In this case, sodium sulfate is split and reacted with ammonia to produce NaOH and (NH4)2SO4. The NaOH is used in the scrubber and the (NH4)2SO4 can be sold as a fertilizer.
[0048] The forth stage is the oxidant stage is used to remove NO, and/or mercury. One embodiment of the oxidant stage would be an integral reaction zone that recirculates an aqueous solution of oxidant and reaction products to effectively remove all the NO, and much of 'the mercury, simultaneously. No sulfur oxides would be removed in this step as they are effectively removed prior to the oxidant stage.
[0049] The fifth stage is the final wash.
[0050] Other embodiments would use 2, 3, 4, 5 or more stages depending upon the pollutants that will be removed and the operating conditions. For example, Stage 1 of the preferred embodiment, would not be required if S03 was not present, Stages 1 and 2 are not required if there is no SO, present, and Stage 5 is not required if species that require a final wash are not present.
The oxidant would be selected depending upon the desired level of removal of NOX and/or Hg.
The oxidant would be selected depending upon the desired level of removal of NOX and/or Hg.
[0051] The following is a partial list of oxidants that are useful for capture of NOX and/or Hg or Hg compounds:
1) Hydrogen Peroxide 2) Hydrogen Peroxide/Nitric Acid Solution (H202/HNO3) 3) Hydrogen Peroxide/Nitric Acid/Hydrochloric Acid Solution (H2O2/HN03/HC1) 4) Sodium Chlorate Solution (NaC103) 5) Sodium Chlorite Solution (NaC102) 6) Sodium Hypochlorite Solution (NaC10) 7) Sodium Perchlorite Solution (NaC104) 8) Chloric Acid Solution (HC103) 9) Oxone Solution (2KHSO5-KHSO4-K2SO4 Triple Salt) 10) Potassium Chlorate Solution (KC103) 11) Potassium Chlorite Solution (KC102) 12) Potassium Hypochlorite Solution (KC10) 13) Potassium Perchlorite Solution (KC104) 14) Potassium Permanganate (KMnO4) 15) Potassium Permanganate/Sodium Hydroxide Solution [0052]Other oxidants or combinations of oxidants are possible.
Further, sodium carbonate and sodium bicarbonate or other alkalis can be substituted for the sodium hydroxide solutions used for pH
adjustment and to provide the ions for complete reactions.
Oxidants can be selected to, remove just NOX, remove just Hg or simultaneously remove both NO, and Hg. Additionally, gaseous oxidants such as ozone, 03, or Chloride dioxide, C102, can be injected into the gas that has had all or most of the SO2 removed.
With proper mixing and sufficient residence, the oxidation of NO
or Hg in the gas phase by gaseous oxidants occurs. Gaseous oxidants are capable of oxidizing NO not only to NO2 but also to N2O5 which rapidly reacts with water or alkaline solutions to form nitric acid or nitrates.
1) Hydrogen Peroxide 2) Hydrogen Peroxide/Nitric Acid Solution (H202/HNO3) 3) Hydrogen Peroxide/Nitric Acid/Hydrochloric Acid Solution (H2O2/HN03/HC1) 4) Sodium Chlorate Solution (NaC103) 5) Sodium Chlorite Solution (NaC102) 6) Sodium Hypochlorite Solution (NaC10) 7) Sodium Perchlorite Solution (NaC104) 8) Chloric Acid Solution (HC103) 9) Oxone Solution (2KHSO5-KHSO4-K2SO4 Triple Salt) 10) Potassium Chlorate Solution (KC103) 11) Potassium Chlorite Solution (KC102) 12) Potassium Hypochlorite Solution (KC10) 13) Potassium Perchlorite Solution (KC104) 14) Potassium Permanganate (KMnO4) 15) Potassium Permanganate/Sodium Hydroxide Solution [0052]Other oxidants or combinations of oxidants are possible.
Further, sodium carbonate and sodium bicarbonate or other alkalis can be substituted for the sodium hydroxide solutions used for pH
adjustment and to provide the ions for complete reactions.
Oxidants can be selected to, remove just NOX, remove just Hg or simultaneously remove both NO, and Hg. Additionally, gaseous oxidants such as ozone, 03, or Chloride dioxide, C102, can be injected into the gas that has had all or most of the SO2 removed.
With proper mixing and sufficient residence, the oxidation of NO
or Hg in the gas phase by gaseous oxidants occurs. Gaseous oxidants are capable of oxidizing NO not only to NO2 but also to N2O5 which rapidly reacts with water or alkaline solutions to form nitric acid or nitrates.
[0053] Bench-scale screening of potential solutions for capturing NOx and Hg was performed using a simple gaseous mixture (Hg + NO +
NO2 + CO2 + H20 + N2 + 02) and an impinger sampling train similar to that described in the American Society of Testing and Materials Method D6784-02 (Ontario Hydro method). Testing has identified solutions that effectively removed both NOx and Hg . The results are shown in the table below:
TABLE 1: BENCH SCALE TEST RESULTS
Solution NO, Removal or NO Hg Removal Conversion to NOa (Hg Total and Hg ) Hydrogen Peroxide Low Low Nitric Acid (40%) + Hydrogen 30 - 40% 30 - 40%
Peroxide Acidified Potassium Permanganate 30 - 40% -100%
Chloric Acid Low 30 - 40%
0.1 M NaC10 pH adjusted to 3.74 -100% -100%
using HC1 0.25 mole/L KMnO4 + 2.5 mole/L NaOH -98% (about 4 ppm 100%
(pH of 11.3) passed through) 0.1 M NaC1O, pH adjusted to 6 75 - 95% -v100%
NaC10 pH adjusted to 5 using HC1 ~70$ --100%
NO2 + CO2 + H20 + N2 + 02) and an impinger sampling train similar to that described in the American Society of Testing and Materials Method D6784-02 (Ontario Hydro method). Testing has identified solutions that effectively removed both NOx and Hg . The results are shown in the table below:
TABLE 1: BENCH SCALE TEST RESULTS
Solution NO, Removal or NO Hg Removal Conversion to NOa (Hg Total and Hg ) Hydrogen Peroxide Low Low Nitric Acid (40%) + Hydrogen 30 - 40% 30 - 40%
Peroxide Acidified Potassium Permanganate 30 - 40% -100%
Chloric Acid Low 30 - 40%
0.1 M NaC10 pH adjusted to 3.74 -100% -100%
using HC1 0.25 mole/L KMnO4 + 2.5 mole/L NaOH -98% (about 4 ppm 100%
(pH of 11.3) passed through) 0.1 M NaC1O, pH adjusted to 6 75 - 95% -v100%
NaC10 pH adjusted to 5 using HC1 ~70$ --100%
[0054] The results show that there are several possible solutions from which to choose. Even the situations that show medium removal ranges such as (Nitric Acid (40%) + Hydrogen Peroxide) or Acidified Potassium Permanganate will remove at higher rates with an appropriate modification to the mass transfer means. The oxidant selected, will then be based on economics, availability, desired level of capture, and/or desired end product.
[0055] Further results are shown on Figures 3 & 4, with Figure 3 illustrating mercury removal as a functioning time using NaC10 at pH 5.73 and Figure 4 illustrating mercury and NOX removal as a function of time using 0.1 M NaC10 solution at pH 8. The proposed reactions with Sodium Hypochlorite (NaOCl) and NO,, and Hg are:
8) 2N0 + 3NaC10 + 2NaOH 2NaNO3 + 3NaC1 + H20 9) 2N0 + 3NaC1O + Na2CO3 2NaNO3 + 3NaC1 + COZi 10) 2N0 + 3NaC10 + 2NaHCO3 ~ 2NaNO3 + 3NaCl + 2C021 + H20 11) 2N02 + NaC1O + 2NaOH --~ 2NaNO3 + NaCl + H20 12) 2NO2 + NaClO + Na2C03 ~ 2NaNO3 + NaCl + C021 13) 2N02 + NaC10 + 2NaHCO3 -* 2NaNO3 + NaCl + 2C021 + H20 14) 2Hg + 4NaClO + 2H20 --+ 2HgC12 + 4NaOH + 02 [0056] In these reactions, an additional source of sodium such as bicarbonate, carbonate or hydroxide is provided to balance the reaction and in order to limit the potentially deleterious reaction of liberating C12 gas. Thus the washing step would not be required. Sodium Chlorite (NaC102), Sodium Chlorate (NaC103) and Sodium Perchlorite (NaC104) can also be used for removal of NO,, and Hg.
8) 2N0 + 3NaC10 + 2NaOH 2NaNO3 + 3NaC1 + H20 9) 2N0 + 3NaC1O + Na2CO3 2NaNO3 + 3NaC1 + COZi 10) 2N0 + 3NaC10 + 2NaHCO3 ~ 2NaNO3 + 3NaCl + 2C021 + H20 11) 2N02 + NaC1O + 2NaOH --~ 2NaNO3 + NaCl + H20 12) 2NO2 + NaClO + Na2C03 ~ 2NaNO3 + NaCl + C021 13) 2N02 + NaC10 + 2NaHCO3 -* 2NaNO3 + NaCl + 2C021 + H20 14) 2Hg + 4NaClO + 2H20 --+ 2HgC12 + 4NaOH + 02 [0056] In these reactions, an additional source of sodium such as bicarbonate, carbonate or hydroxide is provided to balance the reaction and in order to limit the potentially deleterious reaction of liberating C12 gas. Thus the washing step would not be required. Sodium Chlorite (NaC102), Sodium Chlorate (NaC103) and Sodium Perchlorite (NaC104) can also be used for removal of NO,, and Hg.
[0057] The products of the NO,, reactions can be regenerated by the Airborne Process''"' by the reactions:
15) NaNO3 + H20 + NH3 + CO2 --~ NaHC031 + NH4NO3 16) NaCl + H20 + NH3 + CO2 NaHC03 1 + NH4C1 [0058] Although embodiments of the invention have been described above, it is not limited thereto and it will be apparent to those skilled in the art that numerous modifications form part of the present invention insofar as they do not depart from the spirit, nature and scope of the claimed and described invention.
15) NaNO3 + H20 + NH3 + CO2 --~ NaHC031 + NH4NO3 16) NaCl + H20 + NH3 + CO2 NaHC03 1 + NH4C1 [0058] Although embodiments of the invention have been described above, it is not limited thereto and it will be apparent to those skilled in the art that numerous modifications form part of the present invention insofar as they do not depart from the spirit, nature and scope of the claimed and described invention.
Claims (38)
1. A method of scrubbing Hg compounds from a gas stream, comprising: a scrubbing operation, including:
contacting a gas stream containing Hg or Hg compounds and SO x compounds with a sorbent for removing at least a portion of said SO x, compounds present in said stream to provide a partially cleaned gas stream; and contacting said partially cleaned gas stream with an oxidant or oxidant solution to oxidize and/or remove residual Hg or Hg compounds remaining in said stream.
contacting a gas stream containing Hg or Hg compounds and SO x compounds with a sorbent for removing at least a portion of said SO x, compounds present in said stream to provide a partially cleaned gas stream; and contacting said partially cleaned gas stream with an oxidant or oxidant solution to oxidize and/or remove residual Hg or Hg compounds remaining in said stream.
2. The method as set forth in Claim 1, wherein said gas stream includes NO x compounds and a potion of the NO x compounds and/or a portion of the Hg or Hg compounds present in the gas are removed in said scrubbing operation.
3. The method as set forth in Claim 1, wherein said partially cleaned gas stream is further contacted with a second sorbent selected from the group consisting of sodium bicarbonate, sodium carbonate, sodium hydroxide, calcium carbonate, calcium oxide, and calcium hydroxide, magnesium carbonate, magnesium oxide, magnesium hydroxide, buffering agents, additives, organic acids, or combinations thereof to remove substantially all remaining SO x compounds prior to said contacting with an oxidant or oxidant solution.
4. The method as set forth in Claim 1, wherein substantially all of the residual Hg or Hg Compounds are removed from said partially cleaned gas stream.
5. The method as set forth in Claim 2, wherein said partially cleaned gas stream containing NO x compounds is further contacted with a second sorbent selected from the group consisting of sodium bicarbonate, sodium carbonate, sodium hydroxide, calcium carbonate, calcium oxide, and calcium hydroxide, magnesium carbonate, magnesium oxide, magnesium hydroxide, buffering agents, additives, organic acids, or combinations thereof to remove substantially all remaining SO x compounds prior to said contacting with an oxidant.
6. The method as set forth in Claim 2, wherein contacting of said partially cleaned gas stream with an oxidant to remove residual Hg or Hg compounds remaining in said stream further removes at least a portion of NO x in said gas or converts all or part of the NO to NO2.
7. The method as set forth in Claim 6, including contacting said gas containing NO2 with water or an aqueous alkali to remove said NO2 .
8. The method as set forth in Claim 1, including contacting said gas with a final wash.
9. The method as set forth in Claim 1, wherein said oxidant is selected from a group consisting of solutions of hydrogen peroxide, sodium chlorate, sodium chlorite, sodium hypochlorite, sodium perchlorite, chloric acid/sodium chlorate, chloric acid, potassium chlorate, potassium chlorite, potassium hypochlorite, potassium perchlorite, potassium permanganate, or a combination thereof or from a group of gaseous oxidants consisting of ozone, chlorine dioxide, or combination thereof.
10. The method as set forth in Claim 2, wherein said oxidant is selected from a group consisting of solutions of hydrogen peroxide, sodium chlorate, sodium chlorite, sodium hypochlorite, sodium perchlorite, chloric acid/sodium chlorate, chloric acid, potassium chlorate, potassium chlorite, potassium hypochlorite, potassium perchlorite, potassium permanganate, or a combination thereof or from a group of gaseous oxidants consisting of ozone, chlorine dioxide, or combination thereof.
11. The method as set forth in Claim 9, wherein said oxidant is in solution with an acid selected from the group consisting of nitric acid, hydrochloric acid and sulfuric acid.
12. The method as set forth in Claim 9, wherein said oxidant is in solution with an alkali.
13. The method as set forth in Claim 12, wherein said alkali is selected from a group including: caustic soda, sodium carbonate, or sodium bicarbonate.
14. The method as set forth in Claim 9, wherein said oxidant includes chloride ions.
15. The method as set forth in Claim 1, wherein said SO x compounds include SO2 and SO3.
16. The method as set forth in Claim 2, wherein said NO x compounds include NO2, N2O3, N2O5, N x O y and dimers thereof.
17. The method as set forth in Claim 1, further including the step of recirculating unreacted sorbent for use in said scrubbing operation.
18. The method as set forth in Claim 2, further including the step of recirculating unreacted sorbent for use in said scrubbing operation.
19. The method as set forth in Claim 1, wherein said gas is conditioned by injection of sorbent to reduce a portion of the inlet SO3.
20. The method as set forth in Claim 2, wherein said gas is conditioned by injection of sorbent to reduce a portion of the inlet SO3.
21. The method as set forth in Claim 19, wherein at least some of said sulfur dioxide is removed and/or hydrochloric acid, NO x or other acid gases are removed by the said injection.
22. A method of scrubbing NO x compounds from a gas stream containing said NO x compounds comprising a scrubbing operation, including:
contacting a gas stream containing SO x and NO x compounds with a sorbent for removing at least a portion of said SO x compounds present in said stream to provide a partially cleaned gas stream; and contacting said partially cleaned gas stream with an oxidant or oxidant solution to oxidize and/or remove residual NO x remaining in said stream.
contacting a gas stream containing SO x and NO x compounds with a sorbent for removing at least a portion of said SO x compounds present in said stream to provide a partially cleaned gas stream; and contacting said partially cleaned gas stream with an oxidant or oxidant solution to oxidize and/or remove residual NO x remaining in said stream.
23. The method as set forth in Claim 22, wherein at least some of the NO x compounds present in the gas are removed in said scrubbing operation.
24. The method as set forth in Claim 22, wherein said partially cleaned gas is further contacted with a second sorbent selected from the group consisting of sodium bicarbonate, sodium carbonate, sodium hydroxide, calcium carbonate, calcium oxide, calcium hydroxide, magnesium carbonate, magnesium oxide, magnesium hydroxide, buffering agents, additives, organic acids, or combinations thereof to remove substantially all remaining SO x compounds prior to said contacting with an oxidant.
25. The method as set forth in Claim 22, wherein substantially all of the residual NO x Compounds are removed from said partially cleaned gas stream.
26. The method as set forth in Claim 22, wherein oxidation of said partially cleaned gas stream with an oxidant to remove residual NO x remaining in said stream further removes at least a portion of Hg or Hg compounds in said gas.
27. The method as set forth in Claim 22, including contacting said gas containing NO2 with water or an aqueous alkali to remove said NO2.
28. The method as set forth in Claim 22, including contacting said gas with a final wash.
29. The method as set forth in Claim 22, wherein said oxidant is selected from a group consisting of solutions of hydrogen peroxide, sodium chlorate, sodium chlorite, sodium hypochlorite, sodium perchlorite, chloric acid/sodium chlorate, chloric acid, potassium chlorate, potassium chlorite, potassium hypochlorite, potassium perchlorite, potassium permanganate, or a combination thereof or from a group of gaseous oxidants consisting of ozone, chlorine dioxide, or combination thereof.
30. The method as set forth in Claim 29, wherein said oxidant is in solution with an acid selected from the group consisting of nitric acid, hydrochloric acid and sulfuric acid.
31. The method as set forth in Claim 29, wherein said oxidant is in solution with an alkali.
32. The method as set forth in Claim 31, wherein said alkali is selected from a group including: caustic soda, sodium carbonate, or sodium bicarbonate.
33. The method as set forth in Claim 29, wherein said oxidant includes chloride ions.
34. The method as set forth in Claim 22, wherein said gas is conditioned by injection of sorbent to reduce a portion of the inlet SO3.
35. The method as set forth in Claim 22, wherein said gas is conditioned by injection of sorbent to reduce a portion of the inlet SO3.
36. The method as set forth in Claim 35, wherein a portion of said sulfur dioxide is removed and/or hydrochloric acid, NO x or other acid gases are removed by the said injection.
37. The method as forth in claim 2, including contacting said gas with a final wash.
38. The method as set forth in claim 2, wherein said SO x compounds include SO2 and SO3.
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US11/081,612 US7628967B2 (en) | 2002-10-01 | 2005-03-17 | Removal of Hg, NOx, and SOx with using oxidants and staged gas/liquid contact |
US11/081,612 | 2005-03-17 | ||
PCT/CA2006/000407 WO2006096993A1 (en) | 2005-03-17 | 2006-03-15 | Removal of hg, nox and sox using oxidants and staged gas/liquid contact |
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- 2006-03-15 EP EP06721678A patent/EP1901832A4/en not_active Withdrawn
- 2006-03-15 WO PCT/CA2006/000407 patent/WO2006096993A1/en active Application Filing
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2009
- 2009-10-27 US US12/606,834 patent/US8242324B2/en not_active Expired - Fee Related
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CN107525065A (en) * | 2017-08-24 | 2017-12-29 | 管理 | A kind of moisture film spittle condensing vapour utilizes the gas fired-boiler denitration energy-saving appliance of latent heat |
CN109589767A (en) * | 2018-12-17 | 2019-04-09 | 郑州大学 | The method and apparatus of pollutant integration removing in a kind of glass furnace fume |
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US7628967B2 (en) | 2009-12-08 |
EP1901832A1 (en) | 2008-03-26 |
WO2006096993A1 (en) | 2006-09-21 |
US20050214187A1 (en) | 2005-09-29 |
US8242324B2 (en) | 2012-08-14 |
US20100068110A1 (en) | 2010-03-18 |
EP1901832A4 (en) | 2009-03-25 |
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